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991.
Dr. Xiangyuan Ouyang Meifang Wang Linjie Guo Chengjun Cui Ting Liu Yongan Ren Yan Zhao Dr. Zhilei Ge Xiniu Guo Prof. Gang Xie Dr. Jiang Li Prof. Chunhai Fan Prof. Lihua Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(29):11934-11942
Fluorescent copper nanoclusters (CuNCs) have been widely used in chemical sensors, biological imaging, and light-emitting devices. However, individual fluorescent CuNCs have limitations in their capabilities arising from poor photostability and weak emission intensities. As one kind of aggregation-induced emission luminogen (AIEgen), the formation of aggregates with high compactness and good order can efficiently improve the emission intensity, stability, and tunability of CuNCs. Here, DNA nanoribbons, containing multiple specific binding sites, serve as a template for in situ synthesis and assembly of ultrasmall CuNCs (0.6 nm). These CuNC self-assemblies exhibit enhanced luminescence and excellent fluorescence stability because of tight and ordered arrangement through DNA nanoribbons templating. Furthermore, the stable and bright CuNC assemblies are demonstrated in the high-sensitivity detection and intracellular fluorescence imaging of biothiols. 相似文献
992.
Lisi Xie Dr. Jia Tian Yingjie Ouyang Xinai Guo Prof. Dr. Weian Zhang Prof. Dr. Ulf-Peter Apfel Prof. Dr. Wei Zhang Prof. Dr. Rui Cao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):15978-15982
Molecular design to improve catalyst performance is significant but challenging. In enzymes, residue groups that are close to reaction centers play critical roles in regulating activities. Using this bioinspired strategy, three water-soluble polymers were designed with appending Co porphyrins and different side-chain groups to mimic enzyme reaction centers and activity-controlling residue groups, respectively. With these polymers, high hydrogen evolution efficiency was achieved in neutral aqueous media for electro- (turnover frequency >2.3×104 s−1) and photocatalysis (turnover number >2.7×104). Porphyrin units are surrounded and protected by polymer chains, and more importantly, the activity can be tuned with different side-chain groups. Therefore, instead of revising molecular structures that is difficult from both design and synthesis points of view, polymers can be used to improve molecular solubility and stability and simultaneously regulate activity by using side-chain groups. 相似文献
993.
Dr. Lu Jin Fangyuan Cheng Hao Li Prof. Dr. Kui Xie 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):8976-8980
Porous tantalum nitride (Ta3N5) single crystals, combining structural coherence and porous microstructure, would substantially improve the photoelectrochemical performance. The structural coherence would reduce the recombination of charge carriers and maintain excellent transport properties while the porous microstructure would not only reduce photon scattering but also facilitate surface reactions. Here, we grow bulk-porous Ta3N5 single crystals on a two-centimeter scale with (002), (023), and (041) facets, respectively, and show significantly enhanced photoelectrochemical performance. We show the preferential facet growth of porous crystals in a lattice reconstruction strategy in relation to lattice match and lattice channel. We present the facet engineering to enhance light absorption, exciton lifetime and transport properties. The porous Ta3N5 single crystal boosts photoelectrochemical oxidation of alcohols with the (002) facet showing the highest performance of >99 % alcohol conversion and >99 % aldehyde/ketone selectivity. 相似文献
994.
Meng Zhao Dr. Hong-Jie Peng Bo-Quan Li Dr. Xiao Chen Jin Xie Dr. Xinyan Liu Prof. Qiang Zhang Prof. Jia-Qi Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(23):9096-9102
In situ evolution of electrocatalysts is of paramount importance in defining catalytic reactions. Catalysts for aprotic electrochemistry such as lithium–sulfur (Li-S) batteries are the cornerstone to enhance intrinsically sluggish reaction kinetics but the true active phases are often controversial. Herein, we reveal the electrochemical phase evolution of metal-based pre-catalysts (Co4N) in working Li-S batteries that renders highly active electrocatalysts (CoSx). Electrochemical cycling induces the transformation from single-crystalline Co4N to polycrystalline CoSx that are rich in active sites. This transformation propels all-phase polysulfide-involving reactions. Consequently, Co4N enables stable operation of high-rate (10 C, 16.7 mA cm−2) and electrolyte-starved (4.7 μL mgS−1) Li-S batteries. The general concept of electrochemically induced sulfurization is verified by thermodynamic energetics for most of low-valence metal compounds. 相似文献
995.
Bingqing Lin Xi Wu Prof. Dr. Lin Xie Yongqiang Kang Prof. Dr. Hongda Du Prof. Dr. Feiyu Kang Prof. Dr. Jia Li Prof. Dr. Lin Gan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(46):20528-20532
Resolving interstitial hydrogen atoms at the surfaces and interfaces is crucial for understanding the mechanical and physicochemical properties of metal hydrides. Although palladium (Pd) hydrides hold important applications in hydrogen storage and electrocatalysis, the atomic position of interstitial hydrogen at Pd hydride near surfaces still remains undetermined. We report the first direct imaging of subsurface hydrogen atoms absorbed in Pd nanoparticles by using differentiated and integrated differential phase contrast within an aberration-corrected scanning transmission electron microscope. In contrast to the well-established octahedral interstitial sites for hydrogen in the bulk, subsurface hydrogen atoms are directly identified to occupy the tetrahedral interstices. DFT calculations show that the amount and the occupation type of subsurface hydrogen atoms play an indispensable role in fine-tuning the electronic structure and associated chemical reactivity of the Pd surface. 相似文献
996.
Dr. Wei Bai Jingyu Gao Dr. Kun Li Gongrui Wang Dr. Tengfei Zhou Pengju Li Prof. Shengyong Qin Prof. Genqiang Zhang Prof. Zaiping Guo Prof. Chong Xiao Prof. Yi Xie 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(40):17647-17651
Volume expansion and poor conductivity are two major obstacles that hinder the pursuit of the lithium-ion batteries with long cycling life and high power density. Herein, we highlight a misfit compound PbNbS3 with a soft/rigid superlattice structure, confirmed by scanning tunneling microscopy and electrochemical characterization, as a promising anode material for high performance lithium-ion batteries with optimized capacity, stability, and conductivity. The soft PbS sublayers primarily react with lithium, endowing capacity and preventing decomposition of the superlattice structure, while the rigid NbS2 sublayers support the skeleton and enhance the migration of electrons and lithium ions, as a result leading to a specific capacity of 710 mAh g−1 at 100 mA g−1, which is 1.6 times of NbS2 and 3.9 times of PbS. Our finding reveals the competitive strategy of soft/rigid structure in lithium-ion batteries and broadens the horizons of single-phase anode material design. 相似文献
997.
Yun Liu Guangze Yang Song Jin Run Zhang Peng Chen Tengjisi Lianzhou Wang Dong Chen David A. Weitz Chun-Xia Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20240-20249
Understanding drug-release kinetics is critical for the development of drug-loaded nanoparticles. We developed a J-aggregate-based Förster-resonance energy-transfer (FRET) method to investigate the release of novel high-drug-loading (50 wt %) nanoparticles in comparison with low-drug-loading (0.5 wt %) nanoparticles. Single-dye-loaded nanoparticles form J-aggregates because of the high dye-loading (50 wt %), resulting in a large red-shift (≈110 nm) in the fluorescence spectrum. Dual-dye-loaded nanoparticles with high dye-loading using FRET pairs exhibited not only FRET but also a J-aggregate red-shift (116 nm). Using this J-aggregate-based FRET method, dye-core–polymer-shell nanoparticles showed two release processes intracellularly: the dissolution of the dye aggregates into dye molecules and the release of the dye molecules from the polymer shell. Also, the high-dye-loading nanoparticles (50 wt %) exhibited a slow release kinetics in serum and relatively quick release in cells, demonstrating their great potential in drug delivery. 相似文献
998.
Dr. Jun-Dong Yi Dr. Ruikuan Xie Prof. Zai-Lai Xie Prof. Guo-Liang Chai Prof. Tian-Fu Liu Prof. Rui-Ping Chen Prof. Yuan-Biao Huang Prof. Rong Cao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):23849-23856
It is still a great challenge to achieve high selectivity of CH4 in CO2 electroreduction reactions (CO2RR) because of the similar reduction potentials of possible products and the sluggish kinetics for CO2 activation. Stabilizing key reaction intermediates by single type of active sites supported on porous conductive material is crucial to achieve high selectivity for single product such as CH4. Here, Cu2O(111) quantum dots with an average size of 3.5 nm are in situ synthesized on a porous conductive copper-based metal–organic framework (CuHHTP), exhibiting high selectivity of 73 % towards CH4 with partial current density of 10.8 mA cm−2 at −1.4 V vs. RHE (reversible hydrogen electrode) in CO2RR. Operando infrared spectroscopy and DFT calculations reveal that the key intermediates (such as *CH2O and *OCH3) involved in the pathway of CH4 formation are stabilized by the single active Cu2O(111) and hydrogen bonding, thus generating CH4 instead of CO. 相似文献
999.
Yifan Xie Ning Qu Shaobin Lin Haojun Jiang Yanyan Zhang Xiuqing Zhang Hao Liang Fang Chen Xueling Ou 《Electrophoresis》2020,41(12):1095-1102
SNPs, combined with massively parallel sequencing technology, have proven applicability in noninvasive prenatal paternity testing (NIPPT) for singleton pregnancies in our previous research, using circulating cell-free DNA in maternal plasma. However, the feasibility of NIPPT in twin pregnancies has remained uncertain. As a pilot study, we developed a practical method to noninvasively determine the paternity of twin pregnancies by maternal plasma DNA sequencing based on a massively parallel sequencing platform. Blood samples were collected from 15 pregnant women (twin pregnancies at 9–18 weeks of gestation). Parental DNA and maternal plasma cell-free DNA were analyzed with custom-designed probes covering 5226 polymorphic SNP loci. A mathematical model for data interpretation was established, including the zygosity determination and paternity index calculations. Each plasma sample was independently tested against the alleged father and 90 unrelated males. As a result, the zygosity in each twin case was correctly determined, prior to paternity analysis. Further, the correct biological father was successfully identified, and the paternity of all 90 unrelated males was excluded in each case. Our study demonstrates that NIPPT can be performed for twin pregnancies. This finding may contribute to development in NIPPT and diagnosis of certain genetic diseases. 相似文献
1000.
We present a new size-modified Poisson–Boltzmann ion channel (SMPBIC) model and use it to calculate the electrostatic potential, ionic concentrations, and electrostatic solvation free energy for a voltage-dependent anion channel (VDAC) on a biological membrane in a solution mixture of multiple ionic species. In particular, the new SMPBIC model adopts a membrane surface charge density and a natural Neumann boundary condition to reflect the charge effect of the membrane on the electrostatics of VDAC. To avoid the singularity difficulties caused by the atomic charges of VDAC, the new SMPBIC model is split into three submodels such that the solution of one of the submodels is obtained analytically and contains all the singularity points of the SMPBIC model. The other two submodels are then solved numerically much more efficiently than the original SMPBIC model. As an application of this SMPBIC submodel partitioning scheme, we derive a new formula for computing the electrostatic solvation free energy. Numerical results for a human VDAC isoform 1 (hVDAC1) in three different salt solutions, each with up to five different ionic species, confirm the significant effects of membrane surface charges on both the electrostatics and ionic concentrations. The results also show that the new SMPBIC model can describe well the anion selectivity property of hVDAC1, and that the new electrostatic solvation free energy formula can significantly improve the accuracy of the currently used formula. © 2019 Wiley Periodicals, Inc. 相似文献